Following almost a decade with little change in global atmospheric methane mole fraction, we present measurements from the Advanced Global Atmospheric Gases Experiment (AGAGE) and the Australian Commonwealth Scientific and Industrial Research Organisation (CSIRO) networks that show renewed growth starting near the beginning of 2007. Remarkably, a similar growth rate is found at all monitoring locations from this time until the latest measurements. We use these data, along with an inverse method applied to a simple model of atmospheric chemistry and transport, to investigate the possible drivers of the rise. Specifically, the relative roles of an increase in emission rate or a decrease in concentration of the hydroxyl radical, the largest methane sink, are examined. We conclude that: 1) if the annual mean hydroxyl radical concentration did not change, a substantial increase in emissions was required simultaneously in both hemispheres between 2006 and 2007; 2) if a small drop in the hydroxyl radical concentration occurred, consistent with AGAGE methyl chloroform measurements, the emission increase is more strongly biased to the Northern Hemisphere.
Determination of the atmospheric concentrations and lifetime of trichloroethane (CH(3)CCI(3)) is very important in the context of global change. This halocarbon is involved in depletion of ozone, and the hydroxyl radical (OH) concentrations determined from its lifetime provide estimates of the lifetimes of most other hydrogen-containing gases involved in the ozone layer and climate. Global measurements of trichloroethane indicate rising concentrations before and declining concentrations after late 1991. The lifetime of CH(3)CCI(3) in the total atmosphere is 4.8 +/- 0.3 years, which is substantially lower than previously estimated. The deduced hydroxyl radical concentration, which measures the atmosphere's oxidizing capability, shows little change from 1978 to 1994.
[1] Global ozone trends derived from the Stratospheric Aerosol and Gas Experiment I and II (SAGE I/II) combined with the more recent Halogen Occultation Experiment (HALOE) observations provide evidence of a slowdown in stratospheric ozone losses since 1997. This evidence is quantified by the cumulative sum of residual differences from the predicted linear trend. The cumulative residuals indicate that the rate of ozone loss at 35-45 km altitudes globally has diminished. These changes in loss rates are consistent with the slowdown of total stratospheric chlorine increases characterized by HALOE HCl measurements. These changes in the ozone loss rates in the upper stratosphere are significant and constitute the first stage of a recovery of the ozone layer.
[1] The Stratospheric Aerosol and Gas Experiment (SAGE) II V6.1 ozone retrievals are shown to be of better precision at all levels and to be much more accurate than previous retrievals in the lower stratosphere below 20 km altitude. A filtering procedure for removing anomalous ozone profiles associated with volcanic aerosol/cloud effects and other identified artifacts in V6.1 ozone is described. The agreement between SAGE and ozonesondes in the mean is shown to be approximately 10% down to the tropopause. Relative to the sondes, SAGE tends to slightly overestimate ozone (less than 5%) between 15 and 20 km altitude and systematically underestimates ozone in the troposphere by approximately 30% in the regions between 8 km altitude and 2 km below the tropopause. The precisions (random errors) of SAGE ozone retrievals above 25 km altitude are estimated to be 4% or better; they are a factor of 10 worse below 16 km altitude. Linear trends in the differences between coincident SAGE and ozonesondes measurement are generally less than 0.3%/yr and not significantly different from zero in 95% confidence intervals. Compared to V5.96 retrievals, ozone trend differences between 20 and 50 km altitude are approximately 0.1%/yr; below 20 km altitude the SAGE II trends are more positive by approximately 0.2%/yr. For the 1984-1999 period, the SAGE II shows a localized ozone loss of À0.4 ± 0.25%/yr (2s) in the tropics at 20 km altitude. In the lower stratosphere, between 16 and 22 km altitudes, the SAGE shows significant ozone losses in the midlatitudes in both hemispheres during the 1979-1999 periods. The ozone trends range from À0.24 ± 0.18%/yr to À0.77 ± 0.46%/yr (2s). However, in the 1984-1999 period, the downward trends are smaller (À0.07%/yr to À0.25%/yr) in this altitude range, and the trends in the integrated column from 12 to 17 km altitude in midlatitudes (35°-60°) are not significantly different from zero (0.1 ± 0.6%/yr (2s)). Averaged over the tropics (20°S-20°N), the ozone column above 15 km altitude exhibit a trend of À0.12 ± 0.08%/yr (2s).
Thirteen years of Atmospheric Lifetime Experiment/Global Atmospheric Gases Experiment CCl3F and CCl2F2 measurements at five remote, surface, globally distributed sites are analyzed. Comparisons are made against shipboard measurements by the Scripps Institution of Oceanography group and archived air samples collected at Cape Grim, Tasmania, since 1978. CCl3F in the lower troposphere was increasing at an average rate of 9.2 ppt/yr over the period July 1978 to June 1988. CCl2F2 was increasing at an average 17.3 ppt/yr in the lower troposphere over the same period. However, between July 1988 and June 1991 the increases of CCl3F and CCl2F2 in this region have averaged just 7.0 ppt/yr and 15.7 ppt/yr, respectively. The rate of increase has been decreasing 2.4 ppt/yr2 and 2.9 ppt/yr2 over this 3‐year period. Based on a recent scenario of the global releases of these compounds and using the new calibration scale SIO 1993, the equilibrium lifetimes are estimated to be and years for CCl3F and CCl2F2, respectively. Using these lifetime estimates and a two‐dimensional model, it is estimated that global releases of these two chlorofluorocarbons in 1990 were 249±28×106 kg for CCl3F and 366±30×106 kg for CCl2F2. It is also estimated that combined releases of these chlorofluorocarbons in 1990 were 21±5% less than those in 1986.
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